arXiv subjects

D. G. Schlom

Publications and source records attributed to D. G. Schlom.

At least 55 records · Page 3Linked to original sources

arXiv2015

Formation and observation of a quasi-two-dimensional $d_{xy}$ electron liquid in epitaxially stabilized Sr$_{2-x}$La$_{x}$TiO$_{4}$ thin films

We report the formation and observation of an electron liquid in Sr$_{2-x}$La$_{x}$TiO$_4$, the quasi-two-dimensional counterpart of SrTiO$_3$, through reactive molecular-beam epitaxy and {\it in situ} angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3$d_{xy}$ orbitals, analogous to the LaAlO$_3$/SrTiO$_3$ interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling acting co-operatively at similar energy scales, which provides a possible mechanism for explaining the low free carrier concentrations observed at various oxide heterostructures such as the LaAlO$_3$/SrTiO$_3$ interface.

cond-mat.str-el↗

arXiv2015

Spin and lattice excitations of a BiFeO3 thin film and ceramics

We present a comprehensive study of polar and magnetic excitations in BiFeO3 ceramics and a thin film epitaxially grown on an orthorhombic (110) TbScO3 substrate. Infrared reflectivity spectroscopy was performed at temperatures from 5 to 900 K for the ceramics and below room temperature for the thin film. All 13 polar phonons allowed by the factor-group analysis were observed in theceramic samples. The thin-film spectra revealed 12 phonon modes only and an additional weak excitation, probably of spin origin. On heating towards the ferroelectric phase transition near 1100 K, some phonons soften, leading to an increase in the static permittivity. In the ceramics, terahertz transmission spectra show five low-energy magnetic excitations including two which were not previously known to be infrared active; at 5 K, their frequencies are 53 and 56 cm-1. Heating induces softening of all magnetic modes. At a temperature of 5 K, applying an external magnetic field of up to 7 T irreversibly alters the intensities of some of these modes. The frequencies of the observed spin excitations provide support for the recently developed complex model of magnetic interactions in BiFeO3 (R.S. Fishman, Phys. Rev. B 87, 224419 (2013)). The simultaneous infrared and Raman activity of the spin excitations is consistent with their assignment to electromagnons.

cond-mat.mtrl-sci↗

arXiv2015

Stoichiometry Dependence of Potential Screening at La$_{(1-δ)}$Al$_{(1+δ)}$O$_3$/SrTiO$_3$ Interfaces

Hard x-ray photoelectron spectroscopy (HAXPES) and variable kinetic energy x-ray photoelectron spectroscopy (VKE-XPS) analyses have been performed on 10 unit cell La$_{(1-δ)}$Al$_{(1+δ)}$O$_3$ films, with La:Al ratios of 1.1, 1.0, and 0.9, deposited on SrTiO$_3$. Of the three films, only the Al-rich film was known to have a conductive interface. VKE-XPS, coupled with maximum entropy analysis, shows significant differences in the compositional depth profile between the Al-rich, the La-rich, and stoichiometric films; significant La enrichment at the interface is observed in the La-rich and stoichiometric films, while the Al-rich shows little to no intermixing. Additionally, the La-rich and stoichiometric films show a high concentration of Al at the surface, which is not observed in the Al-rich film. HAXPES valence band (VB) analysis shows a broadening of the VB for the Al-rich sample relative to the stoichiometric and La-rich samples, which have insulating interfaces. This broadening is consistent with an electric field across the Al-rich film. These results are consistent with a defect driven electronic reconstruction.

cond-mat.mtrl-sci↗

arXiv2015

Interplay of Spin-Orbit Interactions, Dimensionality, and Octahedral Rotations in Semimetallic SrIrO$_3$

We employ reactive molecular-beam epitaxy to synthesize the metastable perovskite SrIrO$_{3}$ and utilize {\it in situ} angle-resolved photoemission to reveal its electronic structure as an exotic narrow-band semimetal. We discover remarkably narrow bands which originate from a confluence of strong spin-orbit interactions, dimensionality, and both in- and out-of-plane IrO$_6$ octahedral rotations. The partial occupation of numerous bands with strongly mixed orbital characters signals the breakdown of the single-band Mott picture that characterizes its insulating two-dimensional counterpart, Sr$_{2}$IrO$_{4}$, illustrating the power of structure-property relations for manipulating the subtle balance between spin-orbit interactions and electron-electron interactions.

cond-mat.str-el↗

arXiv2014

Correlated vs. conventional insulating behavior in the Jeff=1/2 vs. 3/2 bands in the layered iridate Ba2IrO4

We employ molecular beam epitaxy to stabilize Ba2IrO4 thin films and utilize in situ angle-resolved photoemission spectroscopy to investigate the evolution of its electronic structure through the Neel temperature TN. Our measurements indicate that dispersions of the relativistic Jeff=1/2 and 3/2 bands exhibit an unusual dichotomy in their behavior through the Neel transition. Although the charge gap survives into the paramagnetic state, only the Jeff=1/2 state exhibits a strong temperature dependence and its gap softens with increasing temperature approaching TN, while the nearly fully occupied Jeff=3/2 state which remains nearby in energy exhibits negligible changes with temperature.

cond-mat.str-el↗

arXiv2014

Epitaxial Growth of VO$_{2}$ by Periodic Annealing

We report the growth of ultrathin VO$_{2}$ films on rutile TiO$_{2}$ (001) substrates via reactive molecular-beam epitaxy. The films were formed by the cyclical deposition of amorphous vanadium and its subsequent oxidation and transformation to VO$_{2}$ via solid-phase epitaxy. Significant metal-insulator transitions were observed in films as thin as 2.3 nm, where a resistance change ΔR/R of 25 was measured. Low angle annular dark field scanning transmission electron microscopy was used in conjunction with electron energy loss spectroscopy to study the film/substrate interface and revealed the vanadium to be tetravalent and the titanium interdiffusion to be limited to 1.6 nm.

cond-mat.mtrl-sci↗

arXiv2013

Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO$_3$

We apply ultrafast X-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO$_3$ after above-bandgap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO$_3$: the relevant excited charge carriers must remain localized to be consistent with the data.

cond-mat.mtrl-sci↗

arXiv2013

Structural control of magnetic anisotropy in a strain driven multiferroic EuTiO3 thin film

Octahedral distortion plays a key role in engineering the physical properties of heterostructures composed of perovskite oxides. We observe a strong in-plane uniaxial magnetic anisotropy in a strain-enabled multiferroic EuTiO3 thin film epitaxially grown on a (110)o DyScO3 substrate. First principles calculations show that the magnetic anisotropy is closely correlated with the uniaxial TiO6 octahedral tilting and the ferroelectric polarization of the film, indicating potential strong magnetoelectric coupling in the strain-engineered multiferroic system.

cond-mat.mtrl-sci↗

arXiv2013

Growth and Investigation of Nd_{1-x}Sm_{x}ScO_{3} and Sm_{1-x}Gd_{x}ScO_{3} Solid-Solution Single Crystals

The pseudo-cubic lattice parameters of rare-earth (RE) scandate, REScO3, single crystals grown by the Czochralski technique with RE=Dy to Pr lie between about 3.95 and 4.02 Angstrom. These crystals are the only available perovskite substrates in this lattice constant range that can withstand virtually any thin film growth conditions. Two members of this series, PmScO3 and EuScO3, are, however, not suitable for substrate applications. Because the pseudo-cubic lattice parameters between neighbouring REScO3 compounds decrease with rising atomic number of the RE in about 0.01 Angstrom steps, the unsuitability of PmScO3 (radioactivity) and EuScO3 (incompatibility with Si) causes an interruption in this lattice spacing sequence. To replace them, solid solutions of their adjacent rare-earth scandates, i.e., (Nd0.5Sm0.5)ScO3 and (Sm0.5Gd0.5)ScO3, were grown by the Czochralski method. Their average pseudo-cubic lattice parameters of 3.9979 Angstrom and 3.9784 Angstrom are very close to those of PmScO3 and EuScO3, respectively, and they show very low segregation. These qualities make these solid solutions excellent substitutes for PmScO3 and EuScO3.

cond-mat.mtrl-sci↗

arXiv2013

LaAlO3 stoichiometry found key to electron liquid formation at LaAlO3/SrTiO3 interfaces

Emergent phenomena, including superconductivity and magnetism, found in the two-dimensional electron liquid (2-DEL) at the interface between the insulators LaAlO3 and SrTiO3 distinguish this rich system from conventional two-dimensional electron gases at compound semiconductor interfaces. The origin of this 2-DEL, however, is highly debated with focus on the role of defects in the SrTiO3 while the LaAlO3 has been assumed perfect. Our experiments and first principles calculations show that the cation stoichiometry of the nominal LaAlO3 layer is key to 2-DEL formation: only Al-rich LaAlO3 results in a 2-DEL. While extrinsic defects including oxygen deficiency are known to render LaAlO3/SrTiO3 samples conducting, our results show that in the absence of such extrinsic defects, an interface 2-DEL can form. Its origin is consistent with an intrinsic electronic reconstruction occurring to counteract a polarization catastrophe. This work provides a roadmap for identifying other interfaces where emergent behaviors await discovery.

cond-mat.mtrl-sci↗

arXiv2013

Quasiparticle Mass Enhancement and Temperature Dependence of the Electronic Structure of Ferromagnetic SrRuO3 Thin Films

We report high-resolution angle-resolved photoemission studies of epitaxial thin films of the correlated 4d transition metal oxide ferromagnet SrRuO3. The Fermi surface in the ferromagnetic state consists of well-defined Landau quasiparticles, exhibiting strong coupling to low-energy bosonic modes which contributes to the large effective masses observed by transport and thermodynamic measurements. Upon warming the material through its Curie temperature, we observe a substantial decrease in quasiparticle coherence, but negligible changes in the ferromagnetic exchange splitting, suggesting that local moments play an important role in the ferromagnetism in SrRuO3.

cond-mat.str-el↗

arXiv2012

Temperature dependence of the electronic structure and Fermi-surface reconstruction of Eu(1-x)Gd(x)O through the ferromagnetic metal-insulator transition

We present angle-resolved photoemission spectroscopy of Eu(1-x)Gd(x)O through the ferromagnetic metal-insulator transition. In the ferromagnetic phase, we observe Fermi surface pockets at the Brillouin zone boundary, consistent with density functional theory, which predicts a half metal. Upon warming into the paramagnetic state, our results reveal a strong momentum-dependent evolution of the electronic structure, where the metallic states at the zone boundary are replaced by pseudogapped states at the Brillouin zone center due to the absence of magnetic long-range order of the Eu 4f moments.

cond-mat.str-el↗

arXiv2012

Reversible Control of Magnetic Interactions by Electric Field in a Single Phase Material

Intrinsic magnetoelectric coupling describes the interaction between magnetic and electric polarization through an inherent microscopic mechanism in a single phase material. This phenomenon has the potential to control the magnetic state of a material with an electric field, an enticing prospect for device engineering. We demonstrate 'giant' magnetoelectric cross-field control in a single phase rare earth titanate film. In bulk form, EuTiO3 is antiferromagnetic. However, both anti and ferromagnetic interactions coexist between different nearest neighbor europium ions. In thin epitaxial films, strain can be used to alter the relative strength of the magnetic exchange constants. Here, we not only show that moderate biaxial compression precipitates local magnetic competition, but also demonstrate that the application of an electric field at this strain state, switches the magnetic ground state. Using first principles density functional theory, we resolve the underlying microscopic mechanism resulting in the EuTiO3 G-type magnetic structure and illustrate how it is responsible for the 'giant' cross-field magnetoelectric effect.

cond-mat.mtrl-sci↗

arXiv2012

Magnetodielectric coupling and phonon properties of compressively strained EuTiO3 thin films deposited on LSAT

Compressively strained epitaxial (001) EuTiO3 thin films of tetragonal symmetry have been deposited on (001) (LaAlO3)_0.29-(SrAl_{1/2}Ta_{1/2}O3)_0.71 (LSAT) substrates by reactive molecular-beam epitaxy. Enhancement of the Neel temperature by 1 K with 0.9% compressive strain was revealed. The polar phonons ofthe films have been investigated as a function of temperature and magnetic field by means of infrared reflectance spectroscopy. All three infrared active phonons show strongly stiffened frequencies compared to bulk EuTiO3 in accordance with first principles calculations. The phonon frequencies exhibit gradual softening on cooling leading to an increase in static permittivity. A new polar phonon with frequency near the TO1 soft mode was detected below 150 K. The new mode coupled with the TO1 mode was assigned as the optical phonon from the Brillouin zone edge, which is activated in infrared spectra due to an antiferrodistortive phase transition and due to simultaneous presence of polar and/or magnetic nanoclusters. In the antiferromagnetic phase we have observed a remarkable softening of the lowest-frequency polar phonon under an applied magnetic field, which qualitatively agrees with first principles calculations. This demonstrates the strong spin-phonon coupling in EuTiO3, which is responsible for the pronounced dependence of its static permittivity on magnetic field in the antiferromagnetic phase.

cond-mat.mtrl-sci↗

arXiv2010

Optical Properties of (SrMnO3)n/(LaMnO3)2n superlattices: an insulator-to-metal transition observed in the absence of disorder

We measure the optical conductivity of (SrMnO3)n/(LaMnO3)2n superlattices (SL) for n=1,3,5, and 8 and 10 < T < 400 K. Data show a T-dependent insulator to metal transition (IMT) for n \leq 3, driven by the softening of a polaronic mid-infrared band. At n = 5 that softening is incomplete, while at the largest-period n=8 compound the MIR band is independent of T and the SL remains insulating. One can thus first observe the IMT in a manganite system in the absence of the disorder due to chemical doping. Unsuccessful reconstruction of the SL optical properties from those of the original bulk materials suggests that (SrMnO3)n/(LaMnO3)2n heterostructures give rise to a novel electronic state.

cond-mat.mtrl-sci↗

arXiv2009

Evolution of magnetic phases and orbital occupation in (SrMnO3)n/(LaMnO3)2n superlattices

The magnetic and electronic modifications induced at the interfaces in (SrMnO$_{3}$)$_{n}$/(LaMnO$_{3}$)$_{2n}$ superlattices have been investigated by linear and circular magnetic dichroism in the Mn L$_{2,3}$ x-ray absorption spectra. Together with theoretical calculations, our data demonstrate that the charge redistribution across interfaces favors in-plane ferromagnetic (FM) order and $e_{g}(x^{2}-y^{2})$ orbital occupation, in agreement with the average strain. Far from interfaces, inside LaMnO$_3$, electron localization and local strain favor antiferromagnetism (AFM) and $e_{g}(3z^{2}-r^{2})$ orbital occupation. For $n=1$ the high density of interfacial planes ultimately leads to dominant FM order forcing the residual AFM phase to be in-plane too, while for $n \geq 5$ the FM layers are separated by AFM regions having out-of-plane spin orientation.

cond-mat.str-el↗

arXiv2009

Broadband Dielectric Spectroscopy of Ruddlesden-Popper Sr$_{n+1}$Ti$_{n}$O$_{3n+1}$ ($n$ = 1, 2, 3) Thin Films

We explore the frequency-dependent relative permittivity of Ruddlesden-Popper series Sr(n+1)Ti(n)O(3n+1) (n =1,2,3) thin films as a function of temperature and dc electric field. Interdigitated capacitors and coplanar waveguides were used to extract the frequency response from 500 Hz to 40 GHz. At room temperature, the in-plane relative permittivities obtained for Sr(n+1)Ti(n)O(3n+1) (n =1,2,3) were 42+/-3, 54+/-3, and 77+/-2, respectively, and were independent of frequency. At low temperatures, permittivity increases and electric field tunability develops in Sr(4)Ti(3)O(10).

cond-mat.mtrl-sci↗

arXiv2009

Spin-Charge-Lattice Coupling through Resonant Multi-Magnon Excitations in Multiferroic BiFeO3

Spin-charge-lattice coupling mediated by multi-magnon processes is demonstrated in multiferroic BiFeO3. Experimental evidence of two and three magnons excitations as well as multimagnon coupling at electronic energy scales and high temperatures are reported. Temperature dependent Raman experiments show up to five resonant enhancements of the 2-magnon excitation below the Neel temperature. These are shown to be collective interactions between on-site Fe d-d electronic resonance, phonons and multimagnons

cond-mat.other↗